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1.
Proc Natl Acad Sci U S A ; 119(29): e2113545119, 2022 07 19.
Artículo en Inglés | MEDLINE | ID: mdl-35858330

RESUMEN

Biophysical properties of ligand-gated receptors can be profoundly modified by auxiliary subunits or by the lipid microenvironment of the membrane. Hence, it is sometimes challenging to relate the properties of receptors reconstituted in heterologous expression systems to those of their native counterparts. Here we show that the properties of Caenorhabditis elegans levamisole-sensitive acetylcholine receptors (L-AChRs), the ionotropic acetylcholine receptors targeted by the cholinergic anthelmintic levamisole at neuromuscular junctions, can be profoundly modified by their clustering machinery. We uncovered that L-AChRs exhibit a strong outward rectification in vivo, which was not previously described in heterologous systems. This unusual feature for an ionotropic AChR is abolished by disrupting the interaction of the receptors with the extracellular complex required for their synaptic clustering. When recorded at -60 mV, levamisole-induced currents are similar in the wild type and in L-AChR-clustering-defective mutants, while they are halved in these mutants at more depolarized physiological membrane potentials. Consequently, levamisole causes a strong muscle depolarization in the wild type, which leads to complete inactivation of the voltage-gated calcium channels and to an irreversible flaccid paralysis. In mutants defective for L-AChR clustering, the levamisole-induced depolarization is weaker, allowing voltage-gated calcium channels to remain partially active, which eventually leads to adaptation and survival of the worms. This explains why historical screens for C. elegans mutants resistant to levamisole identified the components of the L-AChR clustering machinery, in addition to proteins required for receptor biosynthesis or efficacy. This work further emphasizes the importance of pursuing ligand-gated channel characterization in their native environment.


Asunto(s)
Antinematodos , Proteínas de Caenorhabditis elegans , Caenorhabditis elegans , Canales de Calcio , Agonistas Colinérgicos , Levamisol , Receptores Colinérgicos , Acetilcolina/metabolismo , Animales , Antinematodos/farmacología , Caenorhabditis elegans/efectos de los fármacos , Caenorhabditis elegans/metabolismo , Proteínas de Caenorhabditis elegans/metabolismo , Canales de Calcio/metabolismo , Agonistas Colinérgicos/farmacología , Levamisol/farmacología , Receptores Colinérgicos/metabolismo
2.
Proc Natl Acad Sci U S A ; 119(39): e2122183119, 2022 Sep 27.
Artículo en Inglés | MEDLINE | ID: mdl-36136968

RESUMEN

Single-molecule electrochemical science has advanced over the past decades and now extends well beyond molecular imaging, to molecular electronics functions such as rectification and amplification. Rectification is conceptually the simplest but has involved mostly challenging chemical synthesis of asymmetric molecular structures or asymmetric materials and geometry of the two enclosing electrodes. Here we propose an experimental and theoretical strategy for building and tuning in situ (in operando) rectification in two symmetric molecular structures in electrochemical environment. The molecules were designed to conduct electronically via either their lowest unoccupied molecular orbital (LUMO; electron transfer) or highest occupied molecular orbital (HOMO; "hole transfer"). We used a bipotentiostat to control separately the electrochemical potential of the tip and substrate electrodes of an electrochemical scanning tunneling microscope (EC-STM), which leads to independent energy alignment of the STM tip, the molecule, and the STM substrate. By creating an asymmetric energy alignment, we observed single-molecule rectification of each molecule within a voltage range of ±0.5 V. By varying both the dominating charge transporting LUMO or HOMO energy and the electrolyte concentration, we achieved tuning of the polarity as well as the amplitude of the rectification. We have extended an earlier proposed theory that predicts electrolyte-controlled rectification to rationalize all the observed in situ rectification features and found excellent agreement between theory and experiments. Our study thus offers a way toward building controllable single-molecule rectifying devices without involving asymmetric molecular structures.

3.
Nano Lett ; 2024 Sep 27.
Artículo en Inglés | MEDLINE | ID: mdl-39329367

RESUMEN

Recent interest in quantum nonlinearity has spurred the development of rectifiers for harvesting energy from ambient radiofrequency waves. However, these rectifiers face efficiency and bandwidth limitations at room temperature. We address these challenges by exploring Bi2Te3, a time-reversal symmetric topological quantum material. Bi2Te3 exhibits robust room temperature second-order voltage generation in both the longitudinal and transverse directions. We harness these coexisting nonlinearities to design a multidirectional quantum rectifier that can simultaneously extract energy from various components of an input signal. We demonstrate the efficacy of Bi2Te3-based rectifiers across a broad frequency range, spanning from existing Wi-Fi bands (2.45 GHz) to frequencies relevant to next-generation 5G technology (27.4 GHz). Our Bi2Te3-based rectifier surpasses previous limitations by achieving a high rectification efficiency and operational frequency, alongside a low operational threshold and broadband functionality. These findings enable practical topological quantum rectifiers for high-frequency electronics and energy conversion, advancing wireless energy harvesting for next-generation communication.

4.
Nano Lett ; 24(25): 7564-7571, 2024 Jun 26.
Artículo en Inglés | MEDLINE | ID: mdl-38809695

RESUMEN

Photocurrents play a crucial role in various applications, including light detection, photovoltaics, and THz radiation generation. Despite the abundance of methods and materials for converting light into electrical signals, the use of metals in this context has been relatively limited. Nanostructures supporting surface plasmons in metals offer precise light manipulation and induce light-driven electron motion. Through the inverse design optimization of a gold nanostructure, we demonstrate enhanced volumetric, unidirectional, intense, and ultrafast photocurrents via a magneto-optical process derived from the inverse Faraday effect. This is achieved through fine-tuning the amplitude, polarization, and gradients in the local light field. The virtually instantaneous process allows dynamic photocurrent modulation by varying optical pulse duration, potentially yielding nanosources of intense, ultrafast, planar magnetic fields and frequency-tunable THz emission. These findings open avenues for ultrafast magnetic material manipulation and hold promise for nanoscale THz spectroscopy.

5.
Nano Lett ; 24(30): 9283-9288, 2024 Jul 31.
Artículo en Inglés | MEDLINE | ID: mdl-39023006

RESUMEN

The electrostatic environment around nanoscale molecular junctions modulates charge transport; solvents alter this environment. Methods to directly probe solvent effects require correlating measurements of the local electrostatic environment with charge transport across the metal-molecule-metal junction. Here, we measure the conductance and current-voltage characteristics of molecular wires using a scanning tunneling microscope-break junction (STM-BJ) setup in two commonly used solvents. Our results show that the solvent environment induces shifts in molecular conductance, which we quantify, but more importantly we find that the solvent also impacts the magnitude of current rectification in molecular junctions. By incorporating electrochemical impedance spectroscopy into the STM-BJ setup, we measure the capacitance of the dipole layer formed at the metal-solvent interface and show that rectification can be correlated with solvent capacitance. These results provide a method of quantifying the impact of the solvent environment and a path toward improved environmental control of molecular devices.

6.
Small ; : e2402188, 2024 Jun 20.
Artículo en Inglés | MEDLINE | ID: mdl-38899397

RESUMEN

Ionic diodes provide ionic current rectification (ICR), which is useful for micro-/nanofluidic devices for ionic current-mediated applications. However, the modulation of ICR is not fully developed, and current challenges include limited active control and localized modulation for further multiplexing of micro-/nanofluidic ionic diodes. Herein, a microfluidic device integrated with particle-assembly-based ionic diodes (PAIDs) and a gas-flow channel above them is presented. Exploiting in-situ gas permeation through a polymeric film, precise control over the physiochemical conditions of the nanopores within the PAIDs, leading to the modulation of ICR is demonstrated. The investigation not only characterizes the rectification properties of the PAIDs but also unveils their capacitor-like behavior and the ability to actively modulate ICR using various gas flows. Furthermore, the reversible modulation of ICR through dynamic switching of gas-dissolved solutions, enabling ion-signal amplification is showcased. This pioneering approach of in situ gas-permeation offers programmable manipulation of ion transport along PAIDs, thereby positioning ionic diodes as versatile nanofluidic components. Looking ahead, the development of multiplexed PAIDs in an addressable manner on a chip holds promise for practical applications across diverse fields, including ion signaling, ion-based logic, chemical reactors, and (bio)chemical sensing.

7.
Small ; 20(40): e2404306, 2024 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-38958070

RESUMEN

Nanofluidic ionic diodes have attracted much attention due to their unique functions as unidirectional ion transportation ability and promising applications from molecular sensing, and energy harvesting to emerging neuromorphic devices. However, it remains a challenge to fabricate diode-like nanofluidic systems with ultrathin film thickness <100 nm. Herein the formation of ultrathin ionic diodes from hybrid nanoassemblies of nanoporous (NP) SiO2 nanofilms and polyelectrolyte layer-by-layer (LbL) multilayers is described. Ultrathin ionic diodes are prepared by integrating polyelectrolyte multilayers onto photo-oxidized NP SiO2 nanofilms obtained from silsesquioxane-containing block copolymer thin films as a template. The obtained ultrathin ionic diodes exhibit ion current rectification (ICR) properties with high ICR factor = ≈20 under low ionic strength and asymmetric pH conditions. It is concluded that this ICR behavior arises from effective ion accumulation and depletion at the interface of NP SiO2 nanofilms and LbL multilayers attributed to high ion selectivity by combining the experimental data and theoretical calculations using finite element methods. These results demonstrate that the hybrid nano assemblies of NP SiO2 nanofilms and polyelectrolyte LbL multilayers have potential applications for (bio)sensing materials and integrated ionic circuits for seamless connection of human-machine interfaces.

8.
Nanotechnology ; 35(36)2024 Jun 18.
Artículo en Inglés | MEDLINE | ID: mdl-38848694

RESUMEN

Thermal rectifiers are essential in optimizing heat dissipation in solid-state devices to enhance energy efficiency, reliability, and overall performance. In this study, we experimentally investigate the thermal rectification phenomenon in suspended asymmetric graphene ribbons (GRs). The asymmetry within the graphene is introduced by incorporating periodic parallel nanoribbons on one side of the GR while maintaining the other side in a pristine form. Our findings reveal a substantial thermal rectification effect in these asymmetric graphene devices, reaching up to 45% at room temperature and increasing further at lower environmental temperatures. This effect is attributed to a significant thermal conductivity contrast between pristine graphene and nanoribbon graphene within the asymmetric structure. We observe that the incorporation of nanoribbons leads to a notable reduction in thermal conductivity, primarily due to phonon scattering and bottleneck effects near the nanoribbon edges. These findings suggest that graphene structures exhibiting asymmetry, facilitated by parallel nanoribbons, hold promise for effective heat management at the nanoscale level and the development of practical phononic devices.

9.
Sensors (Basel) ; 24(18)2024 Sep 20.
Artículo en Inglés | MEDLINE | ID: mdl-39338845

RESUMEN

In this study, we propose a novel rectification method for three cameras using a single image for depth estimation. Stereo rectification serves as a fundamental preprocessing step for disparity estimation in stereoscopic cameras. However, off-the-shelf depth cameras often include an additional RGB camera for creating 3D point clouds. Existing rectification methods only align two cameras, necessitating an additional rectification and remapping process to align the third camera. Moreover, these methods require multiple reference checkerboard images for calibration and aim to minimize alignment errors, but often result in rotated images when there is significant misalignment between two cameras. In contrast, the proposed method simultaneously rectifies three cameras in a single shot without unnecessary rotation. To achieve this, we designed a lab environment with checkerboard settings and obtained multiple sample images from the cameras. The optimization function, designed specifically for rectification in stereo matching, enables the simultaneous alignment of all three cameras while ensuring performance comparable to traditional methods. Experimental results with real camera samples demonstrate the benefits of the proposed method and provide a detailed analysis of unnecessary rotations in the rectified images.

10.
Sensors (Basel) ; 24(16)2024 Aug 22.
Artículo en Inglés | MEDLINE | ID: mdl-39205113

RESUMEN

In broadband terahertz waves generated by femtosecond lasers, spatial chirp will be simultaneously produced with the introduction of angular dispersion. The chirp characteristics of the terahertz wave will directly affect the frequency response, bandwidth response, and intensity response of the terahertz sensor. To enhance the capability of terahertz sensors, it is necessary to control and improve the chirped characteristics of broadband terahertz sources. We generate a chirped terahertz wave via optical rectification in a LiNbO3 prism using the technique of pulse front tilt. The effect of the pump-beam spot size on THz generation is systematically studied. The pump's spot size is manipulated using a telescope system. With a pump spot diameter of 1.8 mm, the scanning spectrum of the THz pulse is narrower and is divided into multiple distinct peaks. In contrast, using a pump spot diameter of 3.7 mm leads to increased efficiency in the generation of THz pulses. Also, we investigate the underlying properties governing the generation of chirped terahertz pulses using varying pump pulse spot diameters.

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